3-5 folds or more amounts of carbon materials are required to fill the capacitance gap between the positive/negative electrodes, which finally restrict the whole energy densities of the devices. To improve electrochemical capacitances of carbon materials, three main strategies have been investigated thoroughly: enlarging specific surface areas, [19] constructing porous structures, [20,21] and introducing pseudocapacitive reactions. [22] But each strategy is not perfect. When the surface areas and the pore volumes are improved, the tap densities of electrodes will be reduced. Moreover, enhancing pseudocapacitance by modifying too many functional groups will decrease the whole conductivity and stability of electrode materials. [23] In the present work, we suggest a new concept of building electron-rich regions on the electrode surface, so as to adsorb more cations and accelerate the charge transfer. As a result, the capacitance of carbon materials will be increased reasonably without sacrificing the density, conductivity, and stability of the whole electrode. However, this idea brings a new challenge because the desired groups with abundant electrons (like phosphate groups) are usually difficult to be modified on the carbon materials. In order to resolve this problem, we used carbon dots (CDs, sub-10 nm) [24,25] with desired groups as the guest, and the commercial polyacrylamide (PAM) hydrogel as the host. After calcination on the host-guest composites, we obtained new carbon frameworks which have abundant electron-rich regions, large surface areas, and appropriate porous structures in the meantime. The optimal sample exhibits a specific capacitance up to 468, 510, and 438 F g −1 in alkaline, acidic, and neutral electrolytes, respectively. When it is fabricated into a hybrid supercapacitors with the positive electrode material Ni(OH) 2 /CNTs using an alkaline electrolyte, the mass ratio of positive/negative electrodes is less than 2, an energy density over 90 Wh kg −1 is realized successfully, and 100% of capacity retention rate is recorded after 10 000 cycles. This material also shows excellent performances in both acidic (PbO 2 as positive electrode) and neutral (LiMn 2 O 4 as positive electrode) systems. Detailed structural characterizations and theoretical calculations prove that the well-preserved phosphate/nitrogen groups from the CDs precursors can effectively modulate the electronic structure and form electron-rich regions on the electrode Hybrid supercapacitors generally show high power and long life spans but inferior energy densities, which are mainly caused by carbon negative electrodes with low specific capacitances. To improve the energy densities, the traditional methods include optimizing pore structures and modifying pseudocapacitive groups on the carbon materials. Here, another promising way is suggested, which has no adverse effects to the carbon materials, that is, constructing electron-rich regions on the electrode surfaces for absorbing cations as much as possible. For this aim, a series of hi...